Background: It is unclear whether walking can decrease cardiovascular disease (CVD) risk or if high intensity physical activity (HIPA) is needed, and whether the association is modified by age. We investigated how sedentary behaviour, walking, and HIPA, were associated with systolic blood pressure (SBP), waist circumference (WC), and low-density lipoprotein cholesterol (LDL-C) among adults and older adults in a general population sample using compositional data analysis. Specifically, the measure of association was quantified by reallocating time between sedentary behaviour and 1) walking, and 2) HIPA. Methods: Cross-sectional data from the fifth examination of the Copenhagen City Heart Study was used. Using the software Acti4, we estimated daily time spent in physical behaviours from accelerometer data worn 24 h/day for 7 days (i.e., right frontal thigh and iliac crest; median wear time: 6 days, 23.8 h/day). SBP, WC, and LDL-C were measured during a physical examination. Inclusion criteria were ≥5 days with ≥16 h of accelerometer recordings per day, and no use of antihypertensives, diuretics or cholesterol lowering medicine. The 24-hour physical behaviour composition consisted of sedentary behaviour, standing, moving, walking, HIPA (i.e., sum of climbing stairs, running, cycling and rowing), and time in bed. We used fitted values from linear regression models to predict the difference in outcome given the investigated time reallocations relative to the group-specific mean composition. Results: Among 1053 eligible participants, we found an interaction between the physical behaviour composition and age. Age-stratified analyses (i.e., </≥65 years; 773 adults, 280 older adults) indicated that less sedentary behaviour and more walking was associated with lower SBP among older adults only. For less sedentary behaviour and more HIPA, the results i) indicated an association with lower SBP irrespective of age, ii) showed an association with a smaller WC among adults, and iii) showed an association with a lower LDL-C in both age groups. Conclusions: Less sedentary behaviour and more walking seems to be associated with lower CVD risk among older adults, while HIPA types are associated with lower risk among adults. Therefore, to reduce CVD risk, the modifying effect of age should be considered in future physical activity-promoting initiatives.